Adhesive compound

ABSTRACT

An adhesive compound consisting essentially of an organic phase and inorganic phase, the organic phase comprising an amorphous aliphatic (co)polymer having a Ring &amp; Ball softening point of between 75 and 180° C., and a second aliphatic material having a Tg of about −5° C. or lower and a kinematic viscosity of 4500 mm 2 /s at 100° C. or less, wherein said organic components are present in weight amounts of between 95/5 and 10/90; the inorganic phase comprising a filler, the filler being present in amount of at least about 15 wt % in the total composition. The compositions are suitable for anti-corrosion coatings or sealants against filtration or penetration of water or moisture. A rubber material may be added to this compound or other anti-corrosion coatings to increase the yield point at high temperatures.

CROSS REFERENCE TO RELATED APPLICATIONS

This application is a divisional of U.S. application Ser. No. 13/141,085filed on 7 Sep. 2011, which is a continuation of PCT application numberPCT/EP2009/067832 filed on 23 Dec. 2009, which claims priority from EPapplication number 08172868.5, filed on 23 Dec. 2008 and U.S.application No. 61/144,748, filed on 15 Jan. 2009. All threeapplications are hereby incorporated by reference in their entireties.

BACKGROUND OF THE INVENTION

1. Field of the Invention

The present invention relates to an adhesive compound, as for example acoating or paste. The compound can be in the form of a tape, like arepair tape, anti-corrosive coating tape or paste in the form of a bar.Dependent on the composition, the paste could also be used as putty andcould be suitably handled by a caulking gun, similar to siliconesealants. More in particular, the present invention relates to the useof an adhesive compound as an anti-corrosive layer or sealant.

2. Description of the Related Art

A tape as anti-corrosive layer is for example described in U.S. Pat. No.5,898,044. This tape comprises a fluid polyisobutene polymer with aglass transition temperature below −40° C. and one or more fillermaterials. Although this material has been useful for example forcoating pipes and covers for manholes, it has still some disadvantages;in particular the behavior at elevated temperature is insufficientbecause this anti-corrosive coating exhibits a runny/dripping behaviorat high temperature. This is a disadvantage because pipes for transportof deep well oil and gas near the well can be at a temperature of 70-85°C. Yet, at other places the coating tape needs to be effective atambient temperature in the ground, but also at high and low (between 50°C. and −40° C.) temperatures at places where the oil pipes are above theground surface or when the coating tape is used to coat man-hole covers.

Anti-corrosive coatings for pipes for transport of oil, gas orpetrochemicals are demanding in view of its anti-corrosive properties,as corrosion due to humidity, as well as corrosion due to anaerobicbacteria has to be precluded.

Other applications may be less demanding, and the polyisobutene basedcoatings tend to be too expensive for a number of other applications.

WO2007/022308 describes a number of hot melt and foam-in-place gasketmaterials comprising a blend of rubber, semicrystalline olefinic polymerand other components. These compositions are described as havingvirtually no tack at room temperature.

BRIEF SUMMARY OF THE INVENTION

It is an object of the invention to provide an adhesive compound withimproved high temperature characteristics.

It is a further object of the invention to provide an adhesive compoundfor use as an anticorrosive coating or paste with improved hightemperature characteristics.

It is another object of this invention, to provide a coating or pastefor use in building, construction, repair and the like as putty, sealantor the like as an alternative to polyisobutene coatings, showing a goodtack to a variety of substrates and being highly impermeable tohumidity/moisture and gas.

It is a further object of the invention to provide a coating or pastefor use as waterproofing material and/or moisture and air and/or gasbarrier.

DESCRIPTION OF ILLUSTRATIVE EMBODIMENTS

The following is a description of certain embodiments of the invention,given by way of example only. One or more of the aforementioned objectsare achieved by providing an adhesive compound consisting essentially ofan organic phase and inorganic phase, the organic phase comprises anamorphous aliphatic (co-)polymer or mixtures thereof having a Ring &Ball softening point of between 75 and 180° C. and a second aliphaticmaterial having a Tg of about −5° C. or less and a kinematic viscosityof 120 mm²/s at 100° C. or less, wherein said organic components arepresent in weight amounts of between 95/5 and 10/90 (polymer to secondmaterial); the inorganic phase comprising a filler, the filler beingpresent in amount of at least about 15 wt % in the total composition.

The adhesive compound allows for very good adhesion, long termstability, self-healing characteristics, chemical resistance, and highimpedance. The compound is therefore very suitable for use as coating,paste, or pressure sensitive adhesive. The compound has very lowpermeability for water or gas. Hence, the compound precludes water toform droplets on a metal surface, nor does it allow anaerobic bacteriato grow. The compound is therefore very suitable for use as coating orpaste in anti-corrosive applications in the oil industry; repair tape inconstruction and the like.

It is thought, that because of the non-fluid character of the polymer,the temperature characteristics with respect to resistance to flow atabout 80 or even 100° C. are substantially improved.

The word adhesive means that at 23° C., the product of the presentinvention is tacky to a substrate at least when the compound is pressedthereto. The compound can get an adhesion sufficient to have thematerial adhere to a surface and when adhered, the compound exhibits acohesive failure.

A suitable test to determine tackiness, is—in analogy to EN 12068—asfollows: a 25 cm long by 5 cm wide strip of material (1.4 to 2 mm thick)is pressed during 10 seconds to a clean steel plate with a 10 kg forceper 1 cm², in such a way that no air is entrapped under the adhesivestrip. Thereafter, the sample is stored for 24 hr at 23° C., and thecompound is tested in a 90° peel test, for example with a tensiletesting machine. The compound according to the present inventionexhibits a cohesive failure, and part of the material stays adhered tothe metal surface. Preferably, the compound is tacky at about 5 kg forceper cm², and even more preferably at 2 kg force per cm².

Generally, the compound of the present invention has pressure sensitiveadhesive characteristics if about 50 wt % or less second aliphaticmaterial is present in the organic phase. The pressure sensitivecharacter is a clear advantage over compositions with fluid polymers, asthe compositions with fluid polymers are always tacky, also if notneeded.

The compound is flexible at room temperature (23° C.). The compoundgenerally has a Tg of about −10° C. or less, more preferably about −20°C. or less, and even more preferably about −30° C. or less.

The Tg can be measured in a rheometer (like for example Physica MCR301), with a PP 8 (plate/plate geometry of 8 mm diameter, with 1 mmlayer of material) and a heating rate of 2° C./min; with a 0.001%deformation and a frequency of 10 rad/s). The temperature at which G″shows a peak can be considered as the Tg. Generally, comparable resultsare obtained with a DSC or DMA. Some materials show more than one peak;generally, the Tg is the peak at the lowest temperature in the spectrum;a man skilled in the art knows which peak is considered the glasstransition temperature.

An advantage of the compound of the present invention is its strength athigh temperature. The compound, in particular if suitable asanti-corrosive coating, according to the present invention is non-fluid,and it appears to be possible to make compounds that keep their shape upto about 100° C. A parameter that is indicative for the high temperatureflow behavior or strength is the yield point. A suitable way ofmeasuring the yield point is in a plate-plate rheometer (as describedabove), in a measurement at elevated temperature (for example 90° C.),with a variable, increasing amplitude, and determining when G′ equalsG″. Polyisobutene materials appear to show a yield point at deformationlower than 1% in a constant frequency sweep (10 rad/s) at 90° C. withincreasing amplitude, whereas the compounds of the present inventiongenerally exhibited a yield point at more than 1% deformation,preferably at about 2% or higher, and even more preferably at about 5%or higher, and even more preferably at about 10% or higher.

In an alternative way, rheological properties were determined on a TAInstruments AR, with a temperature unit and a plate/plate measuringsystem with a spindle of 4.1 cm (1.6 inch) diameter. The distancebetween the plates was in this case 4 mm. With such thicker layer ofmaterial the bulk properties seem to be measured in a more direct way.At 71° C., the polyisobutylene based materials did have a yield pointbelow 0.01% deformation, whereas the materials of the present inventionshowed yield points above 1%. In a preferred embodiment, the materialsof the present invention exhibit a yield point at 71° C. of about 0.1%deformation or higher, preferably at about 0.5% or higher, and mostpreferably at about 1% or higher, if measured in a rheometer with 4 mmplate distance and a 4.1 (1.6 inch) diameter spindle. Temperature sweepswere measured with a strain of 0.005% and an angular frequency of 6.3 Hzover a temperature range of 5 to 90° C. A material based on highmolecular weight polyisobutylene and filler material exhibited at thisvery low strain level, at about 35° C. a G′ equaling G″. At atemperature above about 35° C., G′ appeared to be lower than G″, meaningthat the material behaves as a fluid. In contrast, the materialsaccording the present invention exhibit—at this stress level—always aG′>G″; meaning that this material behaves as a solid.

The compounds of the present invention exhibit besides the good hightemperature characteristics also good tack and adhesive strength. Theadhesive strength of the compound, because of the well balancedcomponents, is such that a cohesive failure is observed.

The compound preferably is used in applications where limited tear forceis applied on the layer of adhesive compound, such as in protectivecoatings, sealants for openings, crevices with low pressureapplications, and ones that can be covered or wrapped with some sort ofmechanical protection.

The amorphous aliphatic polymer generally is an ethene, propene orbutene or higher alkene based polymer. The polymer can be ahomo-polymer, co-polymer or mixtures of these. Copolymers includepolymers from two, three or more monomers, and may be block-co-polymersand/or random copolymers.

Preferred polymers or copolymers are butene or propene-based andpreferably comprise about 30 wt % or more propene or butene polymerizedunits.

Suitable butene based (co)polymers include polyethene-butene,polypropene-butene, polyethylene-isobutene, polyethene-propene-butene,polypropene-butene-hexene and the like.

In a particularly preferred embodiment, an amorphous propene based(co)polymer is used. Such amorphous propene based (co)polymer may bea-tactic polypropylene, co/terpolymers of propylene with other α-olefinshaving 2 to 10 carbon atoms, preferably 2 to 8 carbon atoms, includingethylene, 1-butene, 4-methyl-1-pentene, 1-hexene, 1-heptene, 1-octeneand the like. Such copolymers are known in the art, and have rubberycharacteristics at room temperature.

In a preferred embodiment, a PEPP copolymer is used; such PEPPcopolymers may be random copolymers or block-copolymers, and preferablyis a random copolymer. The amorphous propylene based polymer generallycontains about 40 wt % of propene or more, and even more preferablyabout 60 wt % or more. Generally, the copolymers comprise about 90 wt %or more ethylene and propylene units, preferably about 95 wt % or more,and even more preferably about 98 wt % or more. Other monomer unitspreferably are C4 or higher ethylenically unsaturated compounds, likefor example α,n-butene, isobutene, α,n-hexene, or α,n-octene. Such PEPPcopolymers are known in the art, and commercially available.

In another preferred embodiment, an amorphous polypropylene is used,having about 10 mole % or less comonomers, preferably about 5 mole % orless, and the polypropylene may have substantially no other monomercopolymerized.

Suitable polymers include polymers with a melting point (measured as aR&B softening point) of about 75° C. or higher, preferably about 100° C.or higher, and even more preferable 110° C. or higher. The R&B softeningpoint of the polymers generally will be about 180° C. or lower,preferably 160° C. or lower. The ring and ball softening point can bemeasured according to ASTM E28.

The Tg of the amorphous aliphatic polymer preferably is about −5° C. orlower, preferably −10° C. or more, and even more preferably about −20°C. or lower.

Generally, the polymers will have a Brookfield viscosity according toASTM D3236 at 190° C. of about 20 cP or higher, preferably about 200 cPor higher. Preferably, the viscosity will be about 40,000 cP or lower,more preferably about 10,000 cP or lower.

Preferably, the average molecular weight (Mn in g/mol, as measured withhigh-temperature SEC calibrated with PE-standards; solventtrichlorobenzene; temperature 140° C.; refractive index detector)generally will be about 1,000 or higher, preferably about 2,000 orhigher, and about 100,000 or lower, preferably about 50,000 or lower,and even more preferred about 30,000 or lower. A too low molecularweight may diminish the high temperature characteristics. A too highmolecular weight may cause a lower tack. However, the molecular weightsuitable in certain compositions will depend on the type and/or theamount of polymer, second aliphatic material and the optional othermaterials and may vary.

Preferably, the neat polymer exhibits a penetration depth of about 10.0mm or less, preferably about 5.0 mm or less at 25° C. This hardnesssecures a sufficient strength of the composition of the presentinvention. The penetration depth is measured according to ASTM D5, whichgives the depth in dmm, (tenth of a mm). The most common conditions are100 g penetrating for 5 seconds at a temperature of 25° C. with astandard Needle of 50.8 mm length by 1 mm diameter. Generally, thepenetration depth is about 0.1 mm or more, preferably about 0.3 mm ormore, and even more preferably about 0.7 mm or more, as the polymerpreferably is sufficiently soft to serve as a suitable base material forthe adhesive compound.

The surface tension of such polymers is generally about 22-36 mN/m,preferably about 25 mN/m or more, and preferably about 33 mN/m or less(sessile drop technique using diiodomethane as probe liquid at 20° C.).

The term amorphous is used to describe the macroscopic behavior of thepolymers; the polymer may show micro-crystallinity. The polymer can beconsidered amorphous if the polymer, cooled from the melt without shearor stress applied, exhibits a degree of crystallinity of about 15% orless, preferably about 10% or less, and most preferably about 5% or lesscrystallinity, deduced from a DSC run at a heating rate of 10° C. perminute with reference values taken from the ATHAS database.

Suitable copolymers include Eastoflex® polymers from Eastman Chemical,such as for example Eastoflex® E1003, E1060 or E1200, Vestoplast®polymers from Evonik Degussa, such as for example Vestoplast® 408, 608,703 or 750, or Rextac® polymers from Huntsman, such as for exampleRextac® RT 2730, RT 3535, RT 3585, RT 4460. Suitable amorphous propylenepolymers include Eastoflex® P1010 and P1023 or Rextac® RT 2115, RT 2180.and RT 3180, or Polytac R500 from Crowley Chemicals.

The second major component of the organic phase is an aliphaticmaterial. Aliphatic in this invention comprises linear, branched and/orcycloaliphatic. It is preferred that the second aliphatic material ispredominantly linear or branched as such material may have a lower Tg.

The second aliphatic material has a Tg of about −5° C. or less,preferably about −20° C. or less, and even more preferred about −30° C.or less. The Tg can be measured as described above.

This second aliphatic material generally is a fluid or semicrystallinewaxy solid at room temperature. The second aliphatic material acts as atackyfier

Generally, the molecular weight of this material is about 3000 or less,preferably about 1500 g/mol or less, and more preferably 1000 g/mol orless, preferably 800 g/mol or less. Generally, the molecular weight willbe about 100 g/mol or more, preferably about 200 g/mol or more. If themolecules are mainly linear, generally the molecular weight will be inthe lower range. If branched, like oligomers of butene, the molecularweight can be higher. In case the second compound is a mixture ofmaterials, the average molecular weight confers with the valuesdescribed above, and the polydispersity of each single material isgenerally about 5 or less, and preferably about 3 or lower.

Generally, this material in substantially pure form is molten at 70° C.,and will have a kinematic viscosity at 100° C. of about 4500 mm²/s orlower, preferably about 3000 or lower, and more preferably about 700mm²/s or lower for oligomeric compounds, and of about 120 mm²/s orlower, preferably of about 70 mm²/s or lower for lower molecular weightcompounds. The kinematic viscosity can be measured according to DIN51562. Exemplary kinematic viscosities of Vaseline and of plasticizeroils at 100° C. are in the range of 10 to 15 mm²/s or lower; tackifierresins may show a kinematic viscosity in the range of 30-70 mm²/s.Oligomers, or low molecular weight polymers of butene may have kinematicviscosities up to 4500 mm²/s or less, preferably about 3000 or less, andmore preferably about 700 mm²/s or less

Generally, the second aliphatic material will exhibit a largelyNewtonian fluid behaviour. Hence, such compound (in substantially pureform) will not comprise higher molecular weight compounds that wouldcause the fluid behaviour to become elastic.

In one preferred embodiment of the invention, the second aliphaticmaterial is a polybutene oligomer or polymer. Polybutene is a viscouscopolymer of butene and isobutene monomers. “Polybutene”, as usedherein, refers to both hydrogenated (CAS #68937-10-0) and unhydrogenated(CAS #9003-29-6) forms of the polymer. Polybutene is a viscous,colorless, non-drying, liquid polymer.

The second aliphatic compound is different from the amorphous polymer,thus the compound of the present invention contains at least twodifferent materials in the organic phase. Generally, the amorphouspolymer has a higher viscosity at 100° C. than the second aliphaticmaterial. Furthermore, the second aliphatic material will generallyexhibit a lower molecular weight than the polymer.

Preferably, the amorphous (co)polymer and the second aliphatic materialboth have about the same surface tension. This means that the surfacetension is sufficiently similar that stable mixtures are obtained, andthat no phase separation is observed or expected within a several yearsof use. More preferably, the amorphous polymer and second aliphaticmaterial have such a surface tension that mixtures of these materials atthe targeted mixture ratios do not show visible (by the naked eye) phaseseparation when kept for one month at 100° C.

Preferably, the second aliphatic material has a surface tension of about22-36 mN/m, and more preferably about 25 mN/m or higher, and preferablyabout 33 mN/m or lower.

Preferably, the difference between the surface tension of the polymerand the aliphatic compound is about 7 mN/m or less, more preferably, 5mN/m or less, and even more preferably 3 mN/m or less.

In one preferred embodiment (in particular for use as anti-corrosivecoating in the oil and gas industry), the second aliphatic material issubstantially purely aliphatic or cycloaliphatic. Preferably, the amountof olefinic and/or aromatic groups is low; the amount of olefinic and/oraromatic groups preferably is about 3 mol % or lower, preferably about 2mol % or lower. Furthermore, the material preferably does not containoxygen or nitrogen heteroatoms, hence, the amount of these heteroatomswill be about 2 mol % or lower.

In another preferred embodiment of the invention (in particular for lessdemanding long term uses), the second aliphatic material may comprisehigher amounts of olefinic unsaturation and/or aromatic groups. Theamount preferably is about 20 mol % or less, preferably about 15 mol %or less. Such relatively high amounts can be acceptable when the amountof olefinic unsaturation in the ultimate composition is about 3 mol % orless, preferably about 2 mol % or less.

Suitable second aliphatic materials include wax, purified oil fractions,synthetic oils, paraffinic white oils, white petrolatum and the like.Further suitable materials include low molecular weight polyisobutene,polybutene and low molecular weight resins made by copolymerizing andhydrogenating lower (C4-C8) diolefins with lower (C4-C8) monoolefins orpolymerizing and hydrogenating cyclodiolefins, and the like. Suitableexamples include Penreco® Snow, Penreco® Super, Penreco® Ultima,Penreco® Regent, oil HB 40, Primol® 352, 382, 542 from Exxon, Ondina®15, 32, 46, 68 from Shell, Wingtack® 10 from Cray Valley, Piccotac®1020-E, Regalrez® 1018, Regalite® 1010 from Eastman Chemical, Escorez®2520 from Exxon Mobil.

Suitable polybutenes for use herein include, but are not limited to:Indopol L-14, Molecular Weight (“MW”)=370; Indopol L-50, MW=455; IndopolL-65, MW=435; Indopol L-100, MW=510, H-15, MW=600; H-25, MW=670; H-35,MW=725; H-40, MW=750; H-50, MW=815; H-100, MW=940; H-300, MW=1330;H-1500, MW=2145; H-1900, MW=2270; Panalane L-14E, MW=370; PanalaneH-300E, MW=1330; all trade names of BP Amoco Chemicals (Chicago, Ill.).Other suitable grades of polybutene include Parapol 450, MW=420; Parapol700, MW=700; Parapol 950, MW=950; Parapol 1300, MW=1300; and Parapol2500, MW=2700; all trade names of ExxonMobil Corporation.

The organic phase may further comprise one or more antioxidants,coloring agents, other polymers or oligomers, bitumen,clarifying/nucleating/antistatic agents, flame retardants, acidscavengers, compatibilizers, other plasticizers and the like.

Suitable antioxidants include phenolic antioxidants, phosphites,lactones, thioesters, hydoxylamines, hindered amine light stabilizers(HALS) and other stabilizers.

The amount of the one or more anti-oxidant (relative to the organicphase) may vary, and can be about 4 wt % or less, and is preferablyabout 2 wt % or less. Suitable amounts may be 0.05 wt % or more, andmore preferably between 0.1-1.8 wt %.

In one embodiment, the composition comprises at least one primaryantioxidant. A preferred primary antioxidant comprises stericallyhindered phenol groups. Suitable sterically hindered phenol compoundsare selected from the group consisting of for example Irganox® 1076,Irganox® 1098, Irganox® 1035, Irganox® 1330, Irganox® 1010, Irganox®3114, Irganox® 245, Irganox® MD 1024, Irganox® 259, Irganox® 3125 andthe like. Instead of or in addition to the sterically hindered phenols,sterically hindered alkylthiomethylphenols or arylthiomethylphenols suchas Irganox® 1520 or Irganox® 1726 may be used.

In another preferred embodiment, the composition comprises a mixture ofprimary and secondary antioxidants.

Suitable secondary antioxidants include phosphites and thioesters.According to the invention, suitable phosphites are Irgafos® P-EPQ,Irgafos® 12, Irgafos® 168, Irgafos® 38, Irgafos® 126 and the like.Suitable thioesters may be selected from compounds such as Irganox® PS800, Irganox® PS 802 and the like.

In another preferred embodiment, the composition comprises a mixture ofphenolic-type primary antioxidants phosphite-type secondary antioxidantsand lactone-based antioxidants. Such mixtures are known in the art, andcommercially available, e. g., as Irganox® HP or Irganox® XP blends fromCiba.

In another preferred embodiment, in addition to primary and/or secondaryanti-oxidants, sterically hindered amines may be included in thecomposition. Suitable sterically hindered amines may be selected fromcompounds such as Chemassorb® 2020, Chemassorb® 944, Chemassorb® 119 andthe like.

In yet another preferred embodiment, no antioxidants are added or used.This may be preferred for costs reasons, and may be possible when mixingof the components is performed at reasonable low temperature.

Suitable coloring agents include dyes that are soluble in the organicphase such as for example phthalocyanine pigments. Such dyes may bepresent in a suitable amount to impart sufficient color. Preferably, theamount is about 0.2 to 4 wt % with respect to the organic phase.

The organic phase may further comprise polymeric or oligomeric compoundslike tackifiers, rubbers, polyolefins (other than the first polymer) andthe like. This further material is different from the amorphous polymerand from the second aliphatic material. This further material may beused to improve tack, improve yield strength, lower the Tg and the like.

In one preferred embodiment, the amount of unsaturation in thesepolymers or oligomers is about 4 mol % or lower as too high amounts ofolefinic unsaturation may cause a decrease in stability. Further, thepolymers or oligomers preferably do not comprise substantial amounts ofaromatic groups, like about 4 mol % or less.

In another preferred embodiment, the amount of olefinic unsaturationand/or aromatic groups is higher. The suitability depends much on theend-use, and compounds like SBS rubber may be useful, depending on suchend-use. Suitable amounts of olefinic unsaturation and/or aromaticgroups may be about 8 mol % of the total organic phase or less,preferably about 5 mol % or less, and even more preferred about 2 mol %or less.

The polymeric or oligomeric compound is a different compound than theamorphous aliphatic (co)polymers in the adhesive compound. In onepreferred embodiment, the polymeric compound has a higher molecularweight than the polymer used as amorphous (co)polymer. In anotherpreferred embodiment, the polymeric or oligomeric compound is used toincrease the tackiness of the compound and it has a lower molecularweight than the amorphous (co)polymer.

The polymeric and/or oligomeric compounds are distinguished from thesecond aliphatic material by their higher viscosity and/or softeningpoints (measured as R&B softening point).

Suitable polymers and oligomers include natural rubber, butyl rubber aswell as bromobutyl and chlorobutyl rubber, SBS, SEBS, SIS rubbers (e.g,Kraton® or Vector grades), polyisobutylene polymers (e.g. Opanol® ofBASF or Indopol® polymers of INEOS), fully hydrogenated aliphatic and/orcycloaliphatic hydrocarbon resins (e.g. Escorez® 1304, Escorez® 5380 orRegalite® R1090), Keltan® EPDM or EPM rubbers, or Vistalon® polymersfrom Exxon Chemicals, such as for example Vistalon® 404 or 805 and thelike.

The Mooney viscosities of non crosslinked rubbers (ML 1+8, 125° C.)suitable for the compositions may vary, and can be about 100 or less,and are preferably about 80 or less. Suitable Mooney viscosities (ML1+8, 125° C.) may be 10 or more, and more preferably between 20 and 70.

In another embodiment, a suitable rubber is Kalene® 800 or 1300 fromRoyal elastomers (which are poly(isobutylene-isoprene) polymers with aTg of about −70° C.).

R&B softening points of tackifying hydrocarbon resins suitable for thecompositions may vary, and can be about 150° C. or less, and ispreferably about 120° C. or less. Suitable R&B softening points may be60° C. or more, and more preferably between 80° C. and 115° C.

The amount of this polymeric or oligomeric compound—ifpresent—preferably is present in an amount of about 1 wt % or more,preferably about 2 wt % or more relative to the organic phase.Generally, the amount will be about 40 wt % or less with respect to theorganic phase, preferably about 30 wt % or less and even more preferredabout 25 wt % or less. The amount can be in a range consisting of anycombination of the values stated. Suitable amounts have been shown to bee.g. 5 wt %, 9 wt % and 14 wt %.

Generally, the incorporation of so-called crystallinic polyolefins isless desirable, as they tend to decrease the tack. Such (actually semi-)crystallinic polymers can be polyethylene, isotactic polypropylene andthe like. Hence, preferable, the amount of such semi-crystallinepolymers is less than 5 wt %, preferably less than 3 wt % relative tothe total composition, and such polymers are most preferably notpresent.

It has furthermore been discovered that the strength characteristics ofthe compositions of the present invention at elevated temperature, aswell of those based on liquid polyolefin polymers can be improved withthe use of limited amounts of rubber polymers or other amorphouspolymers with a molecular weight of about 30,000 or more. The molecularweight preferably is about 50,000 or more, and even more preferablyabout 100,000 or more. Rubber polymers include EPDM rubber,polyisoprene, polyisoprene-polyisobutene copolymers, natural rubber,butyl rubber as well as bromobutyl and chlorobutyl rubber, SBS, SEBS,SIS rubbers (e.g, Kraton® or Vector© grades), and the like. It appearedthat olefinic unsaturation in the rubbers did not substantially reducethe long term stability, as the unsaturation is sufficiently isolatedthat little adverse effects were seen. Suitable rubbers includeChlorobutyl 1066 rubber (Exxon Mobil, which is a chlorinatedisobutene/isoprene rubber), Keltan® EPM or EPDM rubber and the like.Also a limited amount of polyisobutene with high molecular weight issuitable to increase the yield point and thereby the high temperaturecharacteristics.

The rubber component is distinguished from the aliphatic polymer by thehigher molecular weight, while having a low glass transitiontemperature. Without wanting to be limited to this theory, it is thoughtthat because of the high molecular weight of the rubber or furthercompound, the polymer chains cause substantial entanglements, andthereby cause a yield point at higher deformation.

The rubber component can be used as non-vulcanized polymer or asslightly crosslinked polymer. The rubber polymer preferably ishomogeneously mixed with the amorphous (co)polymer and the secondaliphatic compound, which would be difficult when the rubber would behighly crosslinked during mixing.

The Mooney viscosities of non crosslinked rubbers (ML 1+8, 125° C.)suitable for the compositions may vary, and can be about 100 or less,and are preferably about 80 or less. Suitable Mooney viscosities (ML1+8, 125° C.) may be 10 or more, and more preferably between 20 and 70.

The amount of rubber material generally in the organic phase is about 1wt % or more, preferably about 2 wt % and even more preferably about 3wt % or more. Generally, the amount is about 30 wt % or less, preferablyabout 25 wt % or less, and even more preferred about 15 wt % or less.

With the use of rubber polymers the yield strength is increased, and theflowability of the composition at elevated temperature is reduced. Withsuch reduction, the useful temperature of the coating is substantiallyincreased up to 85° C. or higher, like for example to about 90° C.

Thus, the present invention also relates to the use of a rubber oraliphatic polymer material with a molecular weight of about 30,000 orhigher in an amount relative to the organic phase, of about 1 wt % ormore, preferably about 2 wt % or more, and an amount of about 30 wt % orless, preferably about 25 wt % or less, to increase the yield strengthof an anti-corrosive coating containing about 20-70 wt % fluidpolyisobutene polymer and about 30-80 wt % inorganic filler. Thepreferred embodiments as described before are particularly suitable inthis embodiment as well.

In another preferred embodiment, the amount of this oligomeric orpolymeric (in particular rubber) compound is less than 5 wt % relativeto the total composition, preferably less than 3 wt %, and is in thisembodiment most preferably not present. A substantial amount of rubbertends to decrease the tack, which may be less preferable, depending onthe application.

The anti-corrosive coating according this invention contains about 20-70wt % fluid polyisobutene polymer and about 30-80 wt % inorganic fillerand a further rubber or aliphatic polymer material with a molecularweight of about 30,000 or higher in an amount relative to the organicphase, of about 1 wt % or more, preferably about 2 wt % or more, and anamount of about 30 wt % or less, preferably about 25 wt % or less. Therubber or aliphatic material aids to increase the yield strength.

The inorganic phase comprises inorganic filler material as majorcomponent. The filler material influences the rheological behavior.

Suitable filler materials are inorganic minerals, salts, oxides andcarbon black. Suitable examples include calcium carbonate, siliconoxide, alumina oxide (which may be in the form of an aluminatrihydrate), titanium dioxide, boron sulphate and (ground) quartz, sand,talc, slate, and bentonite. A preferred filler material is calciumcarbonate.

Suitable filler materials will have an average particle size of about 50μm or lower, preferably of 10 μm or lower, and even more preferred about5 μm or lower. Generally, the average particle size will be about 0.1 μmor more, preferably, about 0.4 μm or more.

The particle size can be measured with laser scattering.

Suitable filler materials may have one particle size and a homogeneousparticle size distribution, or may have two or more particle sizes andtwo or more particle size distributions. Very suitable products may havea particle size distribution such that all particles have a size ofabout 50 μm or less, more preferably about 10 μm or less, and such thatat least 60% of the particles has a size of 0.1 μm or more, preferably,at least about 60 wt % has a size of 0.4 μm or more. In a particularpreferred embodiment, at least about 80 wt % of the particles has a sizeof about 0.6 μm or more.

The filler material preferably is treated to enhance its ability tostably mix with a-polar materials. Generally, filler materials are mademore hydrophobic by surface treatment, for example with fatty acids,fatty alcohols and the like.

Suitable filler materials have a low solubility in water or preferablyabout 0.05 g/1 or less.

The amount of filler in the inorganic phase generally will be about 80wt % or more, preferably about 90 wt % or more, and even more preferablyabout 95 wt % or more.

Suitable filler materials include, but are not limited to Omyalite® 95T,Omyacarb® FT-FL, Omyalite® 90T, Hydrocarb® 95T, Hydrocarb® OG, severalMicrodol® and Finntalc® grades, Micaflor® MF8, Micaflor® MF10, Micaflor®MF25, Mistron® talc, or Talkron® PR-10.

Other materials in the inorganic phase can be colorants, brightener andthe like. Many pigments are inorganic crystalline or amorphousmaterials. It is preferred that the coating comprises a minor amount ofcolorant, such as for example about 5 wt % or less, more preferablyabout 3 wt % or less and maybe even about 1 or 0.5 wt % or less relativeto the inorganic phase. The pigment may be surface treated or thoroughlydispersed in an appropriate liquid to enhance its ability to stably mixwith aliphatic materials. Suitable colors include yellow (e.g, goethite,zinc ferrite), green (e.g, chrome(III)oxide), brown or black (e.g.,magnetite, manganese ferrite), and red (e.g., hematite) or suitablemixtures thereof and additional materials, such as optical brighteners(e. g. titanium dioxide) and the like.

The main components (amorphous (co)polymer, second aliphatic compoundand inorganic filler) of the adhesive compound preferably make up about70 wt % of the compound, preferably about 80 wt % or more, and mostpreferably about 90 wt % or more.

Depending on the required rheological behavior, amounts of thecomponents can be adjusted.

The relative weight amount of organic to inorganic phase generally willbe between about 10/90 to 85/15. Preferably, about 20 wt % or moreorganic phase will be present, preferably about 25 wt % or more.Preferably, the amount of the organic phase will be about 70 wt % orless, preferably about 60 wt % or less. Hence, preferably, the amount ofinorganic phase is about 30 wt % or more, more preferably about 40 wt %or more. Sufficient amount of inorganic material aids in achieving goodrheological behavior and stability.

The amount of amorphous aliphatic (co)polymer to second aliphaticmaterial may vary in certain limits depending on the requiredcharacteristic of the ultimate product and is generally within the rangeof 95/5 to 10/90. For example, a stable well performing anti-corrosivecoating was obtained with a 70/30 mixture of PEPP copolymer andVaseline. In a 30/70 mixture of these components, a paste type ofmaterial was obtained with good fluid and sticky properties. Hence, theamount of polymer relative to the amount of second aliphatic componentpreferably is about 10 wt % or more, preferably about 20 wt % or more.The amount of polymer generally is about 95 wt % or less, preferablyabout 90 wt % or less and even more preferred about 80 wt % or less.

In one embodiment of the invention, the organic phase comprises anamount of amorphous (co)polymer of between about 50-85 wt % and anamount of second aliphatic material of between about 13-40 wt %. Thecomposition preferably comprises an amount of antioxidant of about 0.1wt % or more. In this embodiment the amount of organic phase is about 25to 65, preferably about 25-55 wt % and the amount of inorganic phase isabout 35-75, preferably about 45-75 wt %. This composition is verysuitable for use as anti-corrosive coating, sealant or repair material.The amount of amorphous (co)polymer preferably is about 15 wt % to 45 wt% with respect to the total composition.

The anticorrosive or repair coating preferably is used as a layer on aplastic polymer backing. The backing may be continuous plastic sheet,non-woven or woven material. Suitable materials for the backing includepolyolefin like PP or PE, polyester or polyamide, rubber like EPDM,Kevlar©, PVC, cross-linked thermoplastic polyethylene and UV curingpolyester. In one embodiment, the plastic backing preferably ispolyolefin sheet of material like polyethylene or polypropylene. Inanother embodiment, the backing layer may be polyester (for examplePET), polyamide (for example nylon-6,6) or the like. Polyester sheet ispreferred as backing, as it allows for good printability, is resilientand has good UV resistance.

In a preferred embodiment, the anticorrosive or repair coating is in theform of a tape with a polymer sheet as backing, a layer ofanti-corrosive coating of between 0.1 and 4 mm thick, preferably 0.3-2mm thick, and a non-adhesive removable release liner (like for example asilicon-impregnated film). On application, the release liner is removedand the coating tape is applied with its adhesive coating side to theobject to be coated, and the plastic backing at the outside. Preferably,the tape is about 5 cm (2 inch) or more wide, more preferably about 7.5cm (3 inch) wide or more. Generally, the tape is about 50 cm (20 inch)wide or less, preferably about 25 cm (10 inch) or less.

The tapes of the current invention furthermore, preferably, comprise areinforcing mesh. Such mesh may be woven or non-woven, and suitablematerials include fiber-glass, polyester, nylon, Dyneema®, Twaron®Kevlar®, PP, PE and PVC.

The anti-corrosive or repair coating preferably is produced in the formof a wrap tape in roll form or as a patch and hence used as a layer on arelease liner, preventing the wraps to stick to each other or the patchto stick to a packing material or itself when fold up. The lamination tothe release liner happens in the initial stage of the production processby means of extrusion or calendaring. The release liner has suchcharacteristics that it can easily be removed from the wrap tape uponapplication to a substrate. Suitable release liners are produced fromsilicones, Teflon® or other easy removable polyolefin materials. In asecond stage during the same production process, a meshed carrier and asheet are subsequently applied to the upper part of the wrap tape orpatch, in such way that the meshed carrier will be embodied in the wraptape or patch and the plastic top layer is used as a protective outerlayer. Special rollers will enhance the impregnation of the meshedcarrier into the tape or patch.

In another preferred embodiment of the invention, the organic phasecomprises an amount of amorphous copolymer of between about 20-50 wt %,the amount of second aliphatic material is between about 77-40 wt %. Inthis embodiment the amount of organic phase is about 35-75 wt % and theamount of inorganic phase is 25-65 wt %. This composition is verysuitable for use as paste with excellent tackifying characteristics,combined with anti-corrosive and stability characteristics. Hence, it isvery suitable as putty, sealant or the like.

The adhesive compound of the present invention can be made by mixing theseveral components in a kneader, mixer, extruder or the like. In oneembodiment of the invention, it is preferred to mix the components in akneader under reduced pressure to preclude air entrapment in thecomposition. However, it is also possible to knead at atmosphericpressure. Kneading will cause the temperature to rise.

Preferably the components are mixed at room temperature, and kneaded,where the temperature generally reaches about 50° C. or higher, morepreferably about 70° C. or higher. It is preferred to perform thekneading at a temperature of about 170° C. or lower, preferably about140° C. or lower, and most preferably about 130° C. or lower. Mixing athigher temperatures like at about 180° C. is possible, but may requiremore anti-oxidants to keep stability.

The compositions can be suitably used for coating steel pipes, man-holecovers and the like. The coating compositions can also be used forencapsulating objects containing hazardous components such as objectswith lead containing coatings, asbestos and the like. Such objects canbe successfully encapsulated with the coating according to the presentinvention, as the high impermeability to water and gasses of the coatingwill prevent the hazardous materials to spread into the environment, andthereby making these effectively harmless. Furthermore, the easyapplication allows for minimal surface preparation and therefore minimalenvironmental exposure of the hazardous materials during application.

Other useful applications are the repair of leaks in roofs, pipes forair-conditioning, sewer pipes and the like. The paste can be used tofill cracks, fix windows and the like but also to encapsulate electricalwiring. For example, the compound can be used for the sealing of cableand pipe conduits, cracks and holes to prevent penetration of water

The invention will be elucidated with the following non-limitingexamples.

Example 1

In a kneader, an organic phase consisting of PEPP (Eastoflex® E1060),part of the Vaseline and Omyalite® 95T was added (40 wt % organic phase,60 wt % filler) and the materials were mixed (ultimatelypolymer/Vaseline ratio was 70/30). When homogeneous to the eye theremainder of the Vaseline was added, and the materials were mixed for atotal time of about 2 hr with a highest temperature of about 70° C. Ahomogeneous adhesive compound was obtained. The material was cooled, andthe finished compound was extruded continuously in four strings ofbeads, placed on a 5 cm wide siliconized film. A polyester cloth wasapplied on the beads with the same width as the siliconized film andpressed with a heavy roller or calendaring unit to create sufficientbonding with the compound.

A piece of 5×10 cm was cut from the strip, and the rheological behaviorwas studied (no pressure applied). The material did not show cold flow,nor flow at 50 or 100° C. In contrast, a PIB based material exhibitedflow, in particular above 60° C.

The strip was used to coat 20 cm of a rusty steel pipe, and the adhesivecompound was firmly pressed with hand pressure to the pipe. After oneday, the polyester outer layer was peeled off; the adhesive showedcohesive failure, meaning that the adhesive kept covering the pipe.

Example 2 and Comparative Experiment A

Another batch of material was made according to example 1. This materialwas compared with a PIB based material with 60 wt % filler and 40 wt %Oppanol B 10 SFN from BASF. A cone penetration test was performedaccording to ASTM D217. Results are given in Table 1.

TABLE 1 Comparative Example 2 experiment PP-based PIB-based D217 D217Temperature test Difference test difference 23° C. 66 58 50° C. 95 +44%99 +71% 78° C. 133 +40% 149 +51% (cumulative (cumulative 102%) 157%)

These tests show that the strength of PP based material is substantiallyless sensitive to a temperature increase than polyisobutene basedcoatings.

Example 3

A paste like material was made in an analogous way as the compound ofexample 1, but the amounts were: 70/30 Vaseline/Eastoflex® E1060; and50/50 organic/inorganic phase. The inorganic material was Omyalite® 95T.The paste could be used as putty; and could be suitably handled by acaulking gun, similar to silicone sealants.

Examples 4-6

Three formulations were prepared by thoroughly mixing the components asstated in Table 2.

The compounds of Examples 4 and 5 were prepared in a tilting sigma blademixer; all components but Piccotac® 1020-E were mixed at 170 to 180° C.at about 400 mbar for about 3 hr. Piccotac® was added, and the mixturewas kneaded for another 1.5 hr. A homogeneous adhesive compound wasobtained.

The compound of Example 6 was obtained by mixing all components but theOmyalite® at 70-120° C. at about 400 to 500 mbar. When homogeneous tothe eye, Omyalite® was added, and the mixture was kneaded for anothertwo hr in a temperature range of about 50 to 110° C. at about 400 mbar.A homogeneous adhesive compound was obtained.

Rheological properties were determined on a Physica MCR 301, with a CTD600 temperature unit and a PP 8 measuring system (plate/plate with 8 mmdiameter, and a 1 mm distance between the plates).

Temperature sweeps were done from −70° C. to 90° C. at a deformation of0.001 (which slightly increased up to 0.01%), with a constant frequencyof 10 rad/s, while heating with 2° C./min. Furthermore, amplitude sweepswere done at 90° C. with increasing deformation from 0.001% to 10% at aconstant frequency of 10 rad/s. All three samples showed strong adhesionand cohesive failure of the compound in a 90° peel test. Further resultsare summarized in Table 2.

TABLE 2 Example 4 5 6 Composition Raw Amount Amount Amount materialSupplier in wt % in wt % in wt % Eastoflex ® Eastman 33.5 28.5 — E1003Chemical Eastoflex ® E Eastman — — 34.0 1060 Chemical Piccotac ® Eastman7.3 7.3 — 1020-E Chemical Vaseline Fauth & Co — — 11.3 Chlorobutyl ExxonMobil 8.3 4.0 — rubber 1066 Irganox ® 1010 Ciba 0.9 0.8 0.4 Irgafos ®168 Ciba 0.5 0.4 0.1 Omyalite ® 95T Omya 49.5 59.0 54.1 Rheologicalproperties Measurement Tg Temperature −36° C. −33° C. −33° C. sweepYield point Amplitude >10% >10% 2.5% sweep at Estimated Estimated 90°C.; at % 20-30%  15% deformation

Example 7

In an analogous way to example 1, a compound was prepared from 59.6 wt %CaCO₃ (Omyalite), 29.1 wt % polypropylene (polytac R-500), 11.2 wt %polybutene (Indopol H-300) and 0.1 wt % coloring material. The yieldpoint at 71° C.—measured with an AT instruments as described above,using a gap of 4 mm—was higher than 1%; the high temperaturecharacteristics of this compound were excellent. The tack at roomtemperature was good, the compound showed cohesive failure.

Example 8

In an analogous way to example 1, a compound was prepared from 60.0 wt %CaCO₃ (Omyalite), 25.9 wt % polypropylene (polytac R-500), 14.0 wt %polybutene (Indopol H-300) and 0.1 wt % coloring material. The yieldpoint at 71° C.—measured with an AT instruments as described above,using a gap of 4 mm—was higher than 1%; the high temperaturecharacteristics of this compound were good, and the low temperatureproperties were improved with respect to the material of example 7. Thetack at room temperature was very good, the compound showed cohesivefailure.

Examples 9 and 10

In an analogous way to example 7, compounds were prepared withAl(OH)₃.5H₂O as a filler, and with a mixture of Omyalite and carbonblack. Both compounds showed good properties. The compound withAl(OH)₃.5H₂O exhibited a better gloss, and flame retardant properties.

What is claimed is:
 1. A process for coating a steel pipe or a man holecover, comprising: preparing a compound consisting essentially of anorganic phase and inorganic phase, the organic phase comprising anamorphous aliphatic propene based polymer or copolymer with 30 wt % ormore polymerized propene units and having a Ring & Ball softening pointof between 75 and 180° C., and a second aliphatic material having a Tgof about −5° C. or lower and a kinematic viscosity of 4500 mm²/s at 100°C. or less, wherein said organic components are present in weightamounts of between about 90/10 and about 20/80, said polymer orcopolymer relative to said second material; the inorganic phasecomprising a filler, the filler being present in an amount of at leastabout 30 wt % in the total composition, by mixing components of thecompound at a temperature of about 50° C. or higher, cooling theprepared compound to form a solid compound, applying the solid compoundon a steel pipe or a man hole cover.
 2. The process according to claim1, wherein the step of applying the solid compound comprises applyingthe compound as anti-corrosive coating in the oil and gas industry,repair tape in construction, as an anti-corrosive or repair coating orsealant for steel pipes or for man hole covers.
 3. The process accordingto claim 1, wherein the amorphous aliphatic propene based polymer orcopolymer is a polyethene-polypropene random copolymer or an amorphouspolypropene polymer.
 4. The process according to claim 1, wherein theamorphous aliphatic polymer or copolymer is present in about 15 wt % to45 wt % with respect to the total composition.
 5. The process accordingto claim 1, wherein the amorphous aliphatic polymer or copolymer has oneor more of the following characteristics: (i) the Tg of the amorphousaliphatic polymer or copolymer is about −10° C. or lower, (ii) thepolymer or copolymer has a Brookfield viscosity at 190° C. of about 20cP or higher, the viscosity being about 40,000 cP or lower, (iii) theaverage molecular weight, Mn, as measured with SEC against polyethenestandard, is about 1,000 or higher, and about 100,000 or lower, (iv) theneat polymer or copolymer exhibits a penetration depth of about 10.0 mmor less at 25° C.
 6. The process according to claim 1, wherein thesecond aliphatic material has a molecular weight of about 1500 or lower,and a molecular weight of about 100 or more and wherein the secondaliphatic material is a fluid at room temperature, and has a kinematicviscosity of about 3000 mm²/s or less.
 7. The process according to claim1, wherein the organic phase of the composition further comprisespolymeric or oligomeric compounds, different from the amorphousaliphatic polymer or copolymer and the second aliphatic compound, in anamount of about 2 wt % or more, and an amount of about 30 wt % or less.8. The process according to claim 1, wherein the filler material is atleast one inorganic mineral, salt or oxide, wherein the filler materialhas an average particle size of about 50 μm or lower, and of about 0.1μm or higher.
 9. The process according to claim 8, wherein the fillermaterial is at least one inorganic mineral, salt or oxide, wherein thefiller material has an average particle size of about 10 μm or lower.10. The process according to claim 1, wherein the amorphous aliphaticpolymer or copolymer, second aliphatic compound and inorganic fillerconstitute about 80 wt % or more of the total composition.
 11. Theprocess according to claim 1, wherein the amount of amorphous aliphaticpolymer or copolymer in the organic phase is about 85% or less.
 12. Theprocess according to claim 1, wherein the compound exhibits a yieldpoint at 90° C. at deformations of more than 1% when measured at 10rad/sec with increased deformation.
 13. The process according to claim1, wherein the compound exhibits a cohesive failure when adhered to asurface, when tested: (i) a 25 cm long by 5 cm wide strip of the solidcompound, 1.4 to 2 mm thick, is pressed during 10 seconds to a steelplate with a 5 kg force per 1 cm², in such a way that no air isentrapped under the strip; (ii) thereafter, the sample is stored for 24hr at 23° C., and (iii) the compound is tested in a 90° peel test.
 14. Aprocess for coating a steel pipe, or a man hole cover, comprising:preparing a compound consisting essentially of an organic phase andinorganic phase, the organic phase comprising an amorphous aliphaticpropene based polymer or copolymer with 30 wt % or more polymerizedpropene units and having a Ring & Ball softening point of between 75 and180° C., and a second aliphatic material having a Tg of about −5° C. orlower and a kinematic viscosity of 4500 mm²/s at 100° C. or less,wherein said organic components are present in weight amounts of betweenabout 90/10 and about 20/80, said polymer or copolymer relative to saidsecond material; the inorganic phase comprising a filler, the fillerbeing present in an amount of at least about 30 wt % in the totalcomposition, by mixing components of the compound at a temperature ofabout 50° C. or higher, cooling the prepared compound, applying thecooled compound on a plastic backing and coating the steel pipe or manhole covers with the compound having a plastic backing.
 15. The processaccording to claim 14, wherein the amorphous aliphatic polymer orcopolymer, second aliphatic compound and inorganic filler constituteabout 80 wt % or more of the total composition.
 16. The processaccording to claim 15, wherein the compound exhibits a yield point at90° C. at deformations of more than 1%, when measured at 10 rad/sec withincreased deformation.
 17. The process according to claim 16, whereinthe compound exhibits a cohesive failure when adhered to a surface, whentested: (i) a 25 cm long by 5 cm wide strip of the compound, 1.4 to 2 mmthick, is pressed during 10 seconds to a steel plate with a 5 kg forceper 1 cm², in such a way that no air is entrapped under the strip; (ii)thereafter, the sample is stored for 24 hr at 23° C., and (iii) thecompound is tested in a 90° peel test.
 18. The process according toclaim 17, wherein the filler material is at least one inorganic mineral,salt or oxide, wherein the filler material has an average particle sizeof about 10 μm or lower.
 19. The process according to claim 14, whereinthe compound is applied as a layer on a plastic backing in the form of atape; the plastic backing being polyolefin, polyester or polyamide sheetof material, wherein the compound is between 0.1 and 4 mm thick.
 20. Theprocess of claim 1, wherein the amorphous aliphatic propene basedpolymer or copolymer has a degree of crystallinity of less than 5%.